US12525642B2 - Positive electrode material, and battery - Google Patents

Positive electrode material, and battery

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Publication number
US12525642B2
US12525642B2 US17/902,599 US202217902599A US12525642B2 US 12525642 B2 US12525642 B2 US 12525642B2 US 202217902599 A US202217902599 A US 202217902599A US 12525642 B2 US12525642 B2 US 12525642B2
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positive electrode
solid electrolyte
electrolyte material
battery
electrode active
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US20220416296A1 (en
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Yoshimasa NAKAMA
Masashi Sakaida
Izuru Sasaki
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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Assigned to PANASONIC INTELLECTUAL PROPERTY MANAGEMENT CO., LTD. reassignment PANASONIC INTELLECTUAL PROPERTY MANAGEMENT CO., LTD. ASSIGNMENT OF ASSIGNOR'S INTEREST Assignors: Nakama, Yoshimasa, SAKAIDA, MASASHI, SASAKI, Izuru
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/06—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H01M10/0568—Liquid materials characterised by the solutes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0025—Organic electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/008—Halides
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0088—Composites
    • H01M2300/0091—Composites in the form of mixtures
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0088—Composites
    • H01M2300/0094—Composites in the form of layered products, e.g. coatings
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present disclosure relates to a positive electrode material and a battery.
  • JP 2006-244734 A discloses a battery including, as a solid electrolyte, a compound containing indium as cations and a halogen element as anions. JP 2006-244734 A discloses that, as halogen elements contained in solid electrolytes, chlorine, bromine, and iodine are used, and in particular, chlorine and bromine are preferably used.
  • the present disclosure provides a positive electrode material that can suppress an increase in internal resistance of a battery during charge.
  • a positive electrode material of the present disclosure includes:
  • the present disclosure provides a positive electrode material that can suppress an increase in internal resistance of a battery during charge.
  • FIG. 1 is a cross-sectional view schematically showing the configuration of a positive electrode material 1000 of Embodiment 1.
  • FIG. 2 is a cross-sectional view schematically showing the configuration of the positive electrode material 1000 of Embodiment 1 including a second electrolyte material 100 .
  • FIG. 3 is a cross-sectional view schematically showing the configuration of a battery 2000 of Embodiment 2.
  • FIG. 4 is a cross-sectional view schematically showing the configuration of a battery 3000 of Embodiment 3.
  • JP 2006-244734 A discloses an all-solid-state secondary battery including a solid electrolyte formed of a compound containing indium as cations and a halogen element as anions.
  • JP 2006-244734 A makes the following reference; in this all-solid-state secondary battery, a positive electrode active material has a potential relative to Li of desirably 3.9 V or less on average, and this suppresses generation of a coating formed of a decomposition product resulting from oxidative decomposition of the solid electrolyte, thereby achieving favorable charge and discharge characteristics.
  • JP 2006-244734 A also discloses, as positive electrode active materials having a potential relative to Li of 3.9 V or less on average, general layered transition metal oxides such as LiCoO 2 and LiNi 0.8 CO 0.15 Al 0.05 O 2 .
  • halide solid electrolytes are materials containing, as anions, a halogen element such as fluorine (i.e., F), chlorine (i.e., Cl), bromine (i.e., Br), and iodine (i.e., I).
  • a halogen element such as fluorine (i.e., F), chlorine (i.e., Cl), bromine (i.e., Br), and iodine (i.e., I).
  • a positive electrode material includes a halide solid electrolyte containing at least one element selected from the group consisting of chlorine, bromine, and iodine
  • the halide solid electrolyte is oxidatively decomposed during charge even in the case where a positive electrode active material having a potential relative to Li of 3.9 V or less on average is used.
  • the present inventors discovered a problem that the oxidative decomposition product functions as a resistance layer to increase the internal resistance of the battery during charge.
  • the cause is an oxidation reaction of the at least one element selected from the group consisting of chlorine, bromine, and iodine contained in the halide solid electrolyte.
  • the oxidation reaction refers to a side reaction that occurs in addition to a normal charge reaction in which lithium and electrons are extracted from the positive electrode active material included in the positive electrode material.
  • the side reaction electrons are also extracted from the halide solid electrolyte containing the at least one element in contact with the positive electrode active material, which is selected from the group consisting of chlorine, bromine, and iodine.
  • the positive electrode active material which is selected from the group consisting of chlorine, bromine, and iodine.
  • an oxidative decomposition layer having poor lithium-ion conductivity is formed between the positive electrode active material and the halide solid electrolyte, and the oxidative decomposition layer functions as a large interfacial resistance in an electrode reaction of the positive electrode.
  • chlorine, bromine, and iodine have a relatively large ionic radius and a small interaction force with a cationic component of the halide solid electrolyte, and accordingly are easily oxidized.
  • a positive electrode material includes a positive electrode active material and a solid electrolyte material coating at least partially the positive electrode active material and the solid electrolyte material is a halide solid electrolyte containing fluorine
  • the positive electrode material exhibits excellent oxidation resistance to enable to suppress an increase in internal resistance of a battery including the positive electrode material during charge.
  • the present inventors inferred the reasons as follows; in the case where the halide solid electrolyte contains fluorine having high electronegativity as anions among halogen elements, fluorine is strongly bonded to cations, and accordingly an oxidation reaction of fluorine, that is, a side reaction in which electrons are extracted from fluorine, is less likely to proceed.
  • a fluorine-containing halide solid electrolyte contains lithium (i.e., Li), titanium (i.e., Ti), and M1
  • the fluorine-containing halide solid electrolyte has high lithium-ion conductivity and high oxidation resistance
  • M1 is at least one element selected from the group consisting of calcium (i.e., Ca), magnesium (i.e., Mg), aluminum (i.e., Al), yttrium (i.e., Y), and zirconium (i.e., Zr).
  • the positive electrode material has high oxidation resistance and accordingly can suppress an increase in internal resistance of a battery during charge.
  • the positive electrode material includes a positive electrode active material and a solid electrolyte material coating at least partially the surface of the positive electrode active material, and the solid electrolyte material contains Li, Ti, M1, and F where M1 is at least one element selected from the group consisting of Ca, Mg, Al, Y, and Zr.
  • M1 is at least one element selected from the group consisting of Ca, Mg, Al, Y, and Zr.
  • the solid electrolyte material has high ionic conductivity, the interfacial resistance between the positive electrode active material and the solid electrolyte material can be reduced, thereby improving the output characteristics of the battery.
  • a positive electrode material according to a first aspect of the present disclosure includes:
  • the positive electrode material according to the first aspect has high oxidation resistance. Therefore, the positive electrode material according to the first aspect can suppress an increase in internal resistance of a battery during charge. Also, the first solid electrolyte material has high ionic conductivity. Accordingly, in the positive electrode material, a low interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved. Therefore, the positive electrode material according to the first aspect can improve the output characteristics of the battery.
  • the M1 may include at least one element selected from the group consisting of Mg and Ca.
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include a material represented by the following composition formula (1), Li 6 ⁇ (4 ⁇ 2x1)b1 (Ti 1 ⁇ x1 M1 x1 ) b1 F 6 Formula (1)
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include Li 3 Ti 0.5 Mg 0.5 F 6 .
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include Li 3 Ti 0.5 Ca 0.5 F 6 .
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the M1 may include at least one element selected from the group consisting of Al and Y.
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include a material represented by the following composition formula (2), Li 6 ⁇ (4 ⁇ x2)b2 (Ti 1 ⁇ x2 M1 x2 ) b2 F 6 Formula (2)
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include Li 2.6 Ti 0.4 Al 0.6 F 6 .
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the M1 may include Zr.
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include a material represented by the following composition formula (3), Li 6 ⁇ 4b3 (Ti 1 ⁇ x3 Zr x3 ) b3 F 6 Formula (3)
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the first solid electrolyte material may include Li 3 Ti 0.5 Zr 0.5 F 7 .
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the M1 may include Al and at least one element selected from the group consisting of Mg and Zr.
  • the first solid electrolyte material exhibits higher ionic conductivity. Accordingly, in the positive electrode material, a lower interfacial resistance between the first solid electrolyte material and the positive electrode active material can be achieved.
  • the positive electrode material according to any one of the first to twelfth aspects may further include a second electrolyte material that is a material different from the first solid electrolyte material.
  • resistance derived from migration of Li ions in the positive electrode material can be reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the second electrolyte material may be represented by the following composition formula (5), Li ⁇ M2 ⁇ X ⁇ Formula (5)
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the M2 may include Y.
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the second electrolyte material may include a sulfide solid electrolyte.
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the sulfide solid electrolyte may include lithium sulfide and phosphorus sulfide.
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the sulfide solid electrolyte may be Li 2 S—P 2 S 5 .
  • the ionic conductivity of the second electrolyte material can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material can be further reduced, thereby more effectively suppressing an increase in internal resistance of the battery during charge.
  • the second electrolyte material may be an electrolyte solution including a lithium salt and a solvent.
  • the positive electrode material according to the twentieth aspect can suppress an increase in internal resistance of the battery during charge.
  • the positive electrode active material may include lithium nickel cobalt manganese oxide.
  • the positive electrode material according to the twenty-first aspect can further improve the energy density and the charge and discharge efficiency of the battery.
  • the first solid electrolyte material may be provided between the positive electrode active material and the second electrolyte material.
  • the positive electrode material according to the twenty-second aspect by interposing the first solid electrolyte material having high oxidation resistance between the positive electrode active material and the second electrolyte material, oxidative decomposition of the second electrolyte material can be suppressed, thereby suppressing an increase in internal resistance of the battery during charge.
  • a battery according to a twenty-third aspect of the present disclosure includes:
  • an increase in internal resistance of the battery during charge can be suppressed.
  • the positive electrode material may further include a second electrolyte material that is a material different from the first solid electrolyte material
  • the electrolyte layer may include a material that is the same as the first solid electrolyte material or the same as the second electrolyte material.
  • the battery according to the twenty-fourth aspect has further improved output density and charge and discharge characteristics.
  • the electrolyte layer may include the material that is the same as the first solid electrolyte material.
  • an increase in internal resistance of the battery during charge caused by oxidation of the electrolyte layer is suppressed, thereby further improving the output density and the charge and discharge characteristics.
  • the electrolyte layer may include a first electrolyte layer and a second electrolyte layer, and the first electrolyte layer may be in contact with the positive electrode, and the second electrolyte layer may be in contact with the negative electrode.
  • an increase in internal resistance of the battery during charge can be suppressed.
  • the first electrolyte layer may include a material that is the same as the first solid electrolyte material.
  • the battery according to the twenty-seventh aspect by including the first solid electrolyte material having excellent oxidation resistance in the first electrolyte layer, it is possible to suppress oxidative decomposition of the first electrolyte layer. Therefore, it is possible to suppress an increase in internal resistance of the battery during charge.
  • the second electrolyte layer may include a material that is different from the first solid electrolyte material.
  • the battery according to the twenty-eighth aspect has further improved charge and discharge characteristics.
  • FIG. 1 is a cross-sectional view schematically showing the configuration of a positive electrode material 1000 of Embodiment 1.
  • the positive electrode material 1000 of Embodiment 1 includes a positive electrode active material 110 and a first solid electrolyte material 111 coating at least partially the surface of the positive electrode active material 110 .
  • the first solid electrolyte material 111 includes Li, Ti, M1, and F, and M1 is at least one element selected from the group consisting of Ca, Mg, Al, Y, and Zr.
  • the positive electrode material 1000 has high oxidation resistance. Therefore, the positive electrode material 1000 can suppress an increase in internal resistance of a battery during charge. Also, the first solid electrolyte material 111 has high ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • M1 may be at least one element selected from the group consisting of Ca and Mg.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • the ratio of the amount of substance of Li to the total of the amounts of substance of Ca, Mg, and Ti may be 0.5 or more and 4.5 or less.
  • the first solid electrolyte material 111 may include a material represented by the following composition formula (1).
  • the material represented by the following composition formula (1) may have a crystalline phase. Li 6 ⁇ (4 ⁇ 2x1)b (Ti 1 ⁇ x1 M1 x1 ) b1 F 6 Formula (1),
  • composition formula (1) 0.05 ⁇ x1 ⁇ 0.9 may be satisfied.
  • M1 may be Mg and 0.05 ⁇ x1 ⁇ 0.6 may be satisfied.
  • composition formula (1) 0.80 ⁇ b1 ⁇ 1.71 may be satisfied.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity.
  • the first solid electrolyte material 111 may include Li 3 Ti 0.5 Mg 0.5 F 6 .
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • the first solid electrolyte material 111 may include Li 3 Ti 0.5 Ca 0.5 F 6 .
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • M1 may contain at least one element selected from the group consisting of Al and Y.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • the ratio of the amount of substance of Li to the total of the amounts of substance of Al, Y, and Ti may be 1.7 or more and 4.2 or less.
  • the first solid electrolyte material 111 may include a material represented by the following composition formula (2).
  • the material represented by the composition formula (2) may have a crystalline phase. Li 6 ⁇ (4 ⁇ x2)b2 (Ti 1 ⁇ x2 M1 x2 ) b2 F 6 Formula (2),
  • M1 may be Al.
  • composition formula (2) 0.1 ⁇ x2 ⁇ 0.9 may be satisfied.
  • M1 may be Y and 0.3 ⁇ x2 ⁇ 0.7 may be satisfied.
  • composition formula (2) 0.8 ⁇ b2 ⁇ 1.2 may be satisfied.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity.
  • the first solid electrolyte material 111 may include Li 2.6 Ti 0.4 Al 0.6 F 6 .
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • M1 may include Zr.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • the ratio of the amount of substance of Li to the total of the amounts of substance of Ti and Zr may be 2.0 or more and 6.0 or less.
  • the first solid electrolyte material 111 may include a material represented by the following composition formula (3).
  • the material represented by the composition formula (3) may have a crystalline phase. Li 6 ⁇ 4b3 (Ti 1 ⁇ x3 Zr x3 ) b3 F 6 Formula (3),
  • composition formula (3) 0.1 ⁇ x3 ⁇ 0.8 may be satisfied.
  • composition formula (3) 0.6 ⁇ b3 ⁇ 1.0 may be satisfied.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity.
  • the first solid electrolyte material 111 may include Li 3 Ti 0.5 Zr 0.5 F 7 .
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • M1 may include Al and at least one element selected from the group consisting of Mg and Zr.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity. Accordingly, in the positive electrode material 1000 , a low interfacial resistance between the first solid electrolyte material 111 and the positive electrode active material 110 can be achieved.
  • the ratio of the amount of substance of Li to the total of the amounts of substance of Zr, Mg, Ti, and Al may be 1.33 or more and 3.79 or less.
  • the first solid electrolyte material 111 may include a material represented by the following composition formula (4).
  • the material represented by the composition formula (4) may have a crystalline phase. Li 6 ⁇ (4 ⁇ x4 ⁇ (4 ⁇ m)y)b4 (Ti 1 ⁇ x4 ⁇ y Al x4 M1 y ) b4 F 6 Formula (4),
  • composition formula (4) 0.05 ⁇ x4 ⁇ 0.9 may be satisfied.
  • composition formula (4) 0.05 ⁇ y ⁇ 0.9 may be satisfied.
  • M1 may be Mg and 0.33 ⁇ x4 ⁇ 0.7 may be satisfied.
  • M1 may be Mg and 0.1 ⁇ y ⁇ 0.33 may be satisfied.
  • composition formula (4) 0.8 ⁇ b4 ⁇ 1.2 may be satisfied.
  • the first solid electrolyte material 111 exhibits higher ionic conductivity.
  • the first solid electrolyte material 111 may contain an element other than F as anions.
  • the element contained as the anions include Cl, Br, I, O, S, and Se.
  • the positive electrode material 1000 of Embodiment 1 may further include a second electrolyte material 100 that is a material different from the first solid electrolyte material 111 .
  • the phrase “the second electrolyte material 100 is different from the first solid electrolyte material 111 ” means, for example, that the second electrolyte material 100 has a composition different from that of the first solid electrolyte material 111 , or that the second electrolyte material 100 is in a state different from that of the first solid electrolyte material 111 , for example, is an electrolyte solution.
  • the second electrolyte material 100 may be a material represented by the following composition formula (5). Li ⁇ M2 ⁇ X ⁇ Formula (5),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • metals are B, Si, Ge, As, Sb, and Te.
  • metal elements are all the elements included in Groups 1 to 12 of the periodic table except for hydrogen and all the elements included in Groups 13 to 16 of the periodic table except for B, Si, Ge, As, Sb, Te, C, N, P, O, S, and Se.
  • metaloid elements and metal elements are each a group of elements that can become cations when forming an inorganic compound with a halogen compound.
  • M2 in the second electrolyte material 100 may include Y.
  • the second electrolyte material 100 may include Y as a metal element.
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 including Y may be, for example, a compound represented by a composition formula Li a1 Me b5 Y c X 6 .
  • Me is at least one element selected from the group consisting of a metalloid element and a metal element other than Li and Y.
  • m′ represents the valence of Me.
  • At least one element selected from the group consisting of Mg, Ca, Sr, Ba, Zn, Sc, Al, Ga, Bi, Zr, Hf, Ti, Sn, Ta, and Nb may be used.
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A1). Li 6 ⁇ 3d Y d X 6 Formula (A1),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A2). Li 3 YX 6 Formula (A2),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A3). Li 3 ⁇ 3 ⁇ 1 Y 1+ ⁇ 1 Cl 6 Formula (A3),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A4). Li 3 ⁇ 3 ⁇ 2+a2 Y 1+ ⁇ 2 ⁇ a2 Me a2 Cl 6 ⁇ x5 Br x5 Formula (A4),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A5). Li 3 ⁇ 3 ⁇ 3 Y 1+ ⁇ 3 ⁇ a3 Me a3 Cl 6 ⁇ x6 Br x6 Formula (A5),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A6). Li 3 ⁇ 3 ⁇ 4 ⁇ a4 Y 1+ ⁇ 4 ⁇ a4 Me a4 Cl 6 ⁇ x7 Br x7 Formula (A6),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may be a material represented by the following composition formula (A7). Li 3 ⁇ 3 ⁇ 5 ⁇ 2a5 Y 1+ ⁇ 5 ⁇ a5 Me a5 Cl 6 ⁇ x8 Br x8 Formula( A 7),
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • Li 3 YX 6 Li 2 MgX 4 , Li 2 FeX 4 , Li(Al, Ga, In)X 4 , or Li 3 (Al, Ga, In)X 6 can be used, for example.
  • X includes Cl.
  • an element in a formula is expressed such as “(Al, Ga, In)”
  • this expression indicates at least one element selected from the group of elements in parentheses.
  • the expression “(Al, Ga, In)” is synonymous with the expression “at least one selected from the group consisting of Al, Ga, and In”.
  • the second electrolyte material 100 may be free of sulfur.
  • a sulfide solid electrolyte may be included.
  • the sulfide solid electrolyte which can be used include Li 2 S—P 2 S 5 , Li 2 S—SiS 2 , Li 2 S—B 2 S 3 , Li 2 S—GeS 2 , Li 3.25 Ge 0.25 P 0.75 S 4 , and Li 10 GeP 2 S 12 .
  • LiX, Li 2 O, MO q , Li p MO q , or the like may be added these.
  • X is at least one element selected from the group consisting of F, Cl, Br, and I.
  • M is at least one element selected from the group consisting of P, Si, Ge, B, Al, Ga, In, Fe, and Zn.
  • p and q are each independently a natural number.
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may include lithium sulfide and phosphorus sulfide.
  • the sulfide solid electrolyte may be, for example, Li 2 S—P 2 S 5 .
  • the ionic conductivity of the second electrolyte material 100 can be further increased. Accordingly, resistance derived from migration of Li ions in the positive electrode material 1000 can be further reduced.
  • the second electrolyte material 100 may include an electrolyte solution.
  • the electrolyte solution contains, as a solvent, water or a nonaqueous solvent, and contains a lithium salt dissolved in the solvent.
  • the solvent examples include water, a cyclic carbonate solvent, a linear carbonate solvent, a cyclic ether solvent, a linear ether solvent, a cyclic ester solvent, a linear ester solvent, and a fluorinated solvent.
  • cyclic carbonate solvent examples include ethylene carbonate, propylene carbonate, and butylene carbonate.
  • linear carbonate solvent examples include dimethyl carbonate, ethyl methyl carbonate, and diethyl carbonate.
  • Examples of the cyclic ether solvent include tetrahydrofuran, 1,4-dioxane, and 1,3-dioxolane.
  • linear ether solvent examples include 1,2-dimethoxyethane and 1,2-diethoxyethane.
  • Examples of the cyclic ester solvent include ⁇ -butyrolactone.
  • linear ester solvent examples include methyl acetate.
  • fluorinated solvent examples include fluoroethylene carbonate, methyl fluoropropionate, fluorobenzene, fluoroethyl methyl carbonate, and fluorodimethylene carbonate.
  • solvent one solvent selected from these can be used alone.
  • solvent a combination of two or more solvents selected from these can be used.
  • the electrolyte solution may contain at least one fluorinated solvent selected from the group consisting of fluoroethylene carbonate, methyl fluoropropionate, fluorobenzene, fluoroethyl methyl carbonate, and fluorodimethylene carbonate.
  • lithium salt LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiSO 3 CF 3 , LiN(SO 2 CF 3 ) 2 , LiN(SO 2 C 2 F 5 ) 2 , LiN(SO 2 CF 3 )(SO 2 C 4 Fq), LiC(SO 2 CF 3 ) 3 , or the like can be used.
  • the lithium salt one lithium salt selected from these can be used alone. Alternatively, a mixture of two or more lithium salts selected from these can be used. The concentration of the lithium salt falls within a range of, for example, 0.1 to 15 mol/L.
  • the positive electrode active material 110 includes a material having properties of occluding and releasing metal ions (e.g., lithium ions).
  • metal ions e.g., lithium ions
  • Examples which can be used as the positive electrode active material 110 include a lithium-containing transition metal oxide, a transition metal fluoride, a polyanion material, a fluorinated polyanion material, a transition metal sulfide, a transition metal oxysulfide, and a transition metal oxynitride.
  • the lithium-containing transition metal oxide include Li(Ni, Co, Al)O 2 , Li(Ni, Co, Mn)O 2 , and LiCoO 2 .
  • the lithium-containing transition metal oxide it is possible to reduce the manufacturing costs of the positive electrode material 1000 , and to increase the average discharge voltage.
  • the positive electrode active material 110 may include lithium nickel cobalt manganese oxide.
  • the positive electrode active material 110 may include Li(Ni, Co, Mn)O 2 .
  • the first solid electrolyte material 111 may be provided between the positive electrode active material 110 and the second electrolyte material 100 .
  • the thickness of the first solid electrolyte material 111 coating at least partially the surface of the positive electrode active material 110 may be 1 nm or more and 500 nm or less.
  • the thickness of the first solid electrolyte material 111 is 1 nm or more, a direct contact between the positive electrode active material 110 and the second electrolyte material 100 can be suppressed, thereby suppressing oxidative decomposition of the second electrolyte material 100 . Accordingly, it is possible to improve the charge and discharge efficiency of the battery including the positive electrode material 1000 . In the case where the thickness of the first solid electrolyte material 111 is 500 nm or less, the thickness of the first solid electrolyte material 111 is not excessively large. Accordingly, it is possible to sufficiently reduce the internal resistance of the battery including the positive electrode material 1000 , thereby increasing the energy density of the battery.
  • the method of measuring the thickness of the first solid electrolyte material 111 is not particularly limited.
  • the thickness can be obtained by directly observing the thickness of the first solid electrolyte material 111 with a transmission electron microscope or the like.
  • the mass proportion of the first solid electrolyte material 111 to the positive electrode active material 110 may be 0.01% or more and 30% or less.
  • the mass proportion of the first solid electrolyte material 111 to the positive electrode active material 110 is 0.01% or more, a direct contact between the positive electrode active material 110 and the second electrolyte material 100 can be suppressed, thereby suppressing oxidative decomposition of the second electrolyte material 100 . Accordingly, it is possible to improve the charge and discharge efficiency of the battery including the positive electrode material 1000 . In the case where the mass proportion of the first solid electrolyte material 111 to the positive electrode active material 110 is 30% or less, the thickness of the first solid electrolyte material 111 is not excessively large. Accordingly, it is possible to sufficiently reduce the internal resistance of the battery including the positive electrode material 1000 , thereby increasing the energy density of the battery.
  • the first solid electrolyte material 111 may coat uniformly the surface of the positive electrode active material 110 . Accordingly, a direct contact between the positive electrode active material 110 and the second electrolyte material 100 can be suppressed, thereby suppressing a side reaction of the second electrolyte material 100 . Therefore, it is possible to further improve the charge and discharge characteristics of the battery including the positive electrode material 1000 and to suppress an increase in internal resistance of the battery during charge.
  • the first solid electrolyte material 111 may coat partially the surface of the positive electrode active material 110 .
  • a plurality of positive electrode active materials 110 are in direct contact with each other via their portions which are not covered with the first solid electrolyte material 111 . Accordingly, the electron conductivity between the plurality of positive electrode active materials 110 improves. This enables the battery including the positive electrode material 1000 to operate at a high power.
  • the first solid electrolyte material 111 may coat 30% or more, 60% or more, or 90% or more of the surface of the positive electrode active material 110 .
  • the first solid electrolyte material 111 may coat substantially the entire surface of the positive electrode active material 110 .
  • the surface of the positive electrode active material 110 may be at least partially coated with a coating material that is different from the first solid electrolyte material 111 .
  • the coating material examples include a sulfide solid electrolyte, an oxide solid electrolyte, and a halide solid electrolyte.
  • a sulfide solid electrolyte As the sulfide solid electrolyte and the halide solid electrolyte used as the coating material, the same materials as those exemplified for the second electrolyte material 100 may be used.
  • oxide solid electrolyte used as the coating material examples include a Li—Nb—O compound such as LiNbO 3 , a Li—B—O compound such as LiBC 2 and Li 3 BO 3 , a Li—Al—O compound such as LiAIC 2 , a Li—Si—O compound such as Li 4 SiO 4 , a Li—Ti—O compound such as Li 2 SO 4 and Li 4 Ti 5 O 12 , a Li—Zr—O compound such as Li 2 ZrO 3 , a Li—Mo—O compound such as Li 2 MoO 3 , a Li—V—C compound such as LiV 2 O 5 , a Li—W—O compound such as Li 2 WO 4 , and a Li—P—O compound such as Li 3 PO 4 .
  • Li—Nb—O compound such as LiNbO 3
  • Li—B—O compound such as LiBC 2 and Li 3 BO 3
  • Li—Al—O compound such as LiAIC 2
  • the oxidation resistance of the positive electrode material 1000 can be further improved. Accordingly, an increase in internal resistance of the battery during charge can be suppressed.
  • the positive electrode active material 110 and the first solid electrolyte material 111 may be separated from each other by the coating material so as not to be in direct contact with each other.
  • the oxidation resistance of the positive electrode material 1000 can be further improved. Accordingly, an increase in internal resistance of the battery during charge can be suppressed.
  • the shape of the second electrolyte material 100 of Embodiment 1 is not particularly limited. In the case where the second electrolyte material 100 of Embodiment 1 is a powdery material, its shape may be, for example, acicular, spherical, or ellipsoidal. The shape of the second electrolyte material 100 may be, for example, particulate.
  • the median diameter of the second electrolyte material 100 may be 100 ⁇ m or less.
  • the positive electrode active material 110 and the second electrolyte material 100 can form a favorable dispersion state in the positive electrode material 1000 . This improves the charge and discharge characteristics of the battery including the positive electrode material 1000 .
  • the median diameter of the second electrolyte material 100 may be 10 ⁇ m or less.
  • the median diameter of the second electrolyte material 100 may be smaller than the median diameter of the positive electrode active material 110 .
  • the second electrolyte material 100 and the positive electrode active material 110 can form a more favorable dispersion state in the positive electrode.
  • the median diameter of the positive electrode active material 110 may be 0.1 ⁇ m or more and 100 ⁇ m or less.
  • the positive electrode active material 110 and the second electrolyte material 100 can form a favorable dispersion state in the positive electrode material 1000 . This improves the charge and discharge characteristics of the battery including the positive electrode material 1000 . In the case where the median diameter of the positive electrode active material 110 is 100 ⁇ m or less, the diffusion rate of lithium in the positive electrode active material 110 increases. This enables the battery including the positive electrode material 1000 to operate at a high power.
  • the median diameter of the positive electrode active material 110 may be larger than the median diameter of the second electrolyte material 100 . Accordingly, the positive electrode active material 110 and the second electrolyte material 100 can form a favorable dispersion state.
  • the second electrolyte material 100 and the first solid electrolyte material 111 may be in contact with each other as shown in FIG. 2 .
  • the first solid electrolyte material 111 and the positive electrode active material 110 are in contact with each other.
  • the positive electrode material 1000 of Embodiment 1 may include a plurality of second electrolyte materials 100 and a plurality of positive electrode active materials 110 .
  • the content of the second electrolyte material 100 and the content of the positive electrode active material 110 may be the same, or may be different from each other.
  • the first solid electrolyte material 111 of Embodiment 1 can be manufactured, for example, by the following method.
  • Raw material powders of a binary halide at a blending ratio to obtain a desired composition are prepared.
  • LiF, TiF 4 , and AlF 3 are prepared at a molar ratio of approximately 2.7:0.3:0.7.
  • the blending ratio may be adjusted in advance so as to offset the variation.
  • the raw material powders are well mixed, and then mixed, pulverized, and reacted together by a mechanochemical milling method. Subsequently, the raw material powders may be fired in a vacuum or in an inert atmosphere.
  • the raw material powders may be well mixed, and then fired in a vacuum or in an inert atmosphere.
  • the firing conditions is preferably, for example, firing within a range of 100° C. to 300° C. for 1 hour or more.
  • the firing is performed preferably by sealing the raw material powders in a closed vessel such as a quartz tube.
  • the first solid electrolyte material 111 including a composition such as described above is obtained.
  • the positive electrode material 1000 of Embodiment 1 can be manufactured, for example, by the following method.
  • the positive electrode active material 110 and the first solid electrolyte material 111 are prepared at a predetermined mass ratio.
  • Li(Ni, Co, Mn)O 2 as the positive electrode active material 110 and Li 2.7 Ti 0.3 Al 0.7 F 6 as the first solid electrolyte material 111 are prepared. These two materials are put into the same reaction vessel. A shear force is imparted to the two materials with rotating blades, or a jet stream is used to collide the two materials with each other, for example.
  • the surface of the positive electrode active material Li(Ni, Co, Mn)O 2 can be at least partially coated with Li 2.7 Ti 0.3 Al 0.7 F 6 which is the first solid electrolyte material 111 .
  • a device such as a dry particle composing machine NOBILTA (manufactured by Hosokawa Micron Corporation), a high-speed flow impact machine (manufactured by Nara Machinery Co., Ltd.), or a jet mill.
  • NOBILTA dry particle composing machine
  • a high-speed flow impact machine manufactured by Nara Machinery Co., Ltd.
  • a jet mill a jet mill.
  • the positive electrode material 1000 including the positive electrode active material Li(Ni, Co, Mn)O 2 whose surface is at least partially coated with Li 2.7 Ti 0.3 Al 0.7 F 6 which is the first solid electrolyte material 111 .
  • Embodiment 2 will be described below. The description overlapping with that of Embodiment 1 will be omitted as appropriate.
  • FIG. 3 is a cross-sectional view schematically showing the configuration of a battery 2000 of Embodiment 2.
  • the battery 2000 of Embodiment 2 includes a positive electrode 201 , an electrolyte layer 202 , and a negative electrode 203 .
  • the positive electrode 201 includes the positive electrode material 1000 of Embodiment 1.
  • the electrolyte layer 202 is disposed between the positive electrode 201 and the negative electrode 203 .
  • v1 represents, when the total volume of the positive electrode material 1000 and the second electrolyte material 100 included in the positive electrode 201 is defined as 100 , the volume ratio of the positive electrode material 1000 .
  • v1 represents, when the total volume of the positive electrode material 1000 and the second electrolyte material 100 included in the positive electrode 201 is defined as 100 , the volume ratio of the positive electrode material 1000 .
  • 30 ⁇ v1 a sufficient energy density of the battery can be achieved.
  • v1 ⁇ 98 is satisfied, the battery 2000 can operate at a high power.
  • the thickness of the positive electrode 201 may be 10 ⁇ m or more and 500 ⁇ m or less. In the case where the thickness of the positive electrode 201 is 10 ⁇ m or more, a sufficient energy density of the battery can be achieved. In the case where the thickness of the positive electrode 201 is 500 ⁇ m or less, the battery 2000 can operate at a high power.
  • the electrolyte layer 202 includes an electrolyte material.
  • the electrolyte material may be, for example, a third solid electrolyte material.
  • the electrolyte layer 202 may be a solid electrolyte layer.
  • the third solid electrolyte material a material that is the same as the first solid electrolyte material 111 of Embodiment 1 or the same as the second electrolyte material 100 of Embodiment 1 may be used.
  • the electrolyte layer 202 may include a material that is the same as the first solid electrolyte material 111 of Embodiment 1 or the same as the second electrolyte material 100 of Embodiment 1.
  • the output density and the charge and discharge characteristics of the battery 2000 can be further improved.
  • the same material as the first solid electrolyte material 111 of Embodiment 1 may be used.
  • the electrolyte layer 202 may include the same material as the first solid electrolyte material 111 of Embodiment 1.
  • a halide solid electrolyte As the third solid electrolyte material included in the electrolyte layer 202 , a halide solid electrolyte, a sulfide solid electrolyte, an oxide solid electrolyte, a polymer solid electrolyte, or a complex hydride solid electrolyte may be used.
  • Examples which can be used as the oxide solid electrolyte of the third solid electrolyte material include: a NASICON solid electrolyte typified by LiTi 2 (PO 4 ) 3 and element-substituted substances thereof; a (LaLi)TiO 3 -based perovskite solid electrolyte; a LISICON solid electrolyte typified by Li 14 ZnGe 4 O 16 , Li 4 SiO 4 , and LiGeO 4 and element-substituted substances thereof; a garnet solid electrolyte typified by Li 7 La 3 Zr 2 O 12 and element-substituted substances thereof; Li 3 PO 4 and N-substituted substances thereof; and glass and glass ceramics that include a Li—B—O compound such as LiBO 2 or Li 3 BO 3 as a base and to which Li 2 SO 4 , Li 2 CO 3 , or the like is added.
  • a Li—B—O compound such as LiBO 2 or Li 3 BO 3 as
  • Examples which can be used as the polymer solid electrolyte of the third solid electrolyte material include a compound of a polymer compound and a lithium salt.
  • the polymer compound may have an ethylene oxide structure.
  • a polymer compound having an ethylene oxide structure can contain a large amount of a lithium salt. Accordingly, the ionic conductivity can be further increased.
  • Examples which can be used as the lithium salt include LiPF 6 , LiBF 4 , LiSbF 6 , LiAsF 6 , LiSO 3 CF 3 , LiN(SO 2 CF 3 ) 2 , LiN(SO 2 C 2 F 5 ) 2 , LiN(SO 2 CF 3 )(SO 2 C 4 Fq), and LiC(SO 2 CF 3 ) 3 .
  • One lithium salt selected from the exemplified lithium salts can be used alone. Alternatively, a mixture of two or more lithium salts selected from the exemplified lithium salts can be used.
  • Examples which can be used as the complex hydride solid electrolyte of the third solid electrolyte material include LiBH 4 —LiI and LiBH 4 —P 2 S 5 .
  • the electrolyte layer 202 may include the third solid electrolyte material as its main component.
  • the electrolyte layer 202 may include the third solid electrolyte material, for example, at a mass proportion of 50% or more (i.e., 50 mass % or more) with respect to the entire electrolyte layer 202 .
  • the electrolyte layer 202 may include the third solid electrolyte material, for example, at a mass proportion of 70% or more (i.e., 70 mass % or more) with respect to the entire electrolyte layer 202 .
  • the charge and discharge characteristics of the battery 2000 can be further improved.
  • the electrolyte layer 202 may include the third solid electrolyte material as its main component and further include inevitable impurities, a starting material used for synthesis of the third solid electrolyte material, a by-product, a decomposition product, etc.
  • the electrolyte layer 202 may include the third solid electrolyte material, for example, at a mass proportion of 100% (i.e., 100 mass %) with respect to the entire electrolyte layer 202 , except for inevitably incorporated impurities.
  • the charge and discharge characteristics of the battery 2000 can be further improved.
  • the electrolyte layer 202 may consist of the third solid electrolyte material.
  • the electrolyte layer 202 may include two or more of the materials listed as the third solid electrolyte material.
  • the electrolyte layer 202 may include a halide solid electrolyte and a sulfide solid electrolyte.
  • the thickness of the electrolyte layer 202 may be 1 ⁇ m or more and 300 ⁇ m or less. In the case where the thickness of the electrolyte layer 202 is 1 ⁇ m or more, a short circuit between the positive electrode 201 and the negative electrode 203 is less likely to occur. In the case where the thickness of the electrolyte layer 202 is 300 ⁇ m or less, the battery 2000 can operate at a high power.
  • the negative electrode 203 includes a material having properties of occluding and releasing metal ions (e.g., lithium ions).
  • the negative electrode 203 includes, for example, a negative electrode active material.
  • Examples which can be used as the negative electrode active material include a metal material, a carbon material, an oxide, a nitride, a tin compound, and a silicon compound.
  • the metal material may be an elemental metal. Alternatively, the metal material may be an alloy. Examples of the metal material include lithium metal and a lithium alloy.
  • Examples of the carbon material include natural graphite, coke, semi-graphitized carbon, a carbon fiber, spherical carbon, artificial graphite, and amorphous carbon. From the viewpoint of capacity density, silicon, tin, a silicon compound, or a tin compound can be used.
  • the negative electrode 203 may include a solid electrolyte material.
  • the solid electrolyte material the solid electrolyte materials exemplified as the materials of the electrolyte layer 202 may be used. With the above configuration, the lithium-ion conductivity inside the negative electrode 203 can be improved, and accordingly the battery 2000 can operate at a high power.
  • the median diameter of the negative electrode active material particles may be 0.1 ⁇ m or more and 100 ⁇ m or less. In the case where the median diameter of the negative electrode active material particles is 0.1 ⁇ m or more, the negative electrode active material particles and the solid electrolyte material can form a favorable dispersion state in the negative electrode. This improves the charge and discharge characteristics of the battery 2000 . In the case where the median diameter of the negative electrode active material particles is 100 ⁇ m or less, diffusion of lithium in the negative electrode active material particles is fast. This enables the battery 2000 to operate at a high power.
  • the median diameter of the negative electrode active material particles may be larger than the median diameter of the solid electrolyte material included in the negative electrode 203 . Thus, a favorable dispersion state of the negative electrode active material particles and the solid electrolyte material can be formed.
  • v2 represents, when the total volume of the negative electrode active material particles and the solid electrolyte material included in the negative electrode 203 is defined as 100 , the volume ratio of the negative electrode active material particles.
  • v2 represents, when the total volume of the negative electrode active material particles and the solid electrolyte material included in the negative electrode 203 is defined as 100 , the volume ratio of the negative electrode active material particles.
  • v2 ⁇ 95 a sufficient energy density of the battery can be achieved.
  • the battery 2000 can operate at a high power.
  • the thickness of the negative electrode 203 may be 10 ⁇ m or more and 500 ⁇ m or less. In the case where the thickness of the negative electrode 203 is 10 ⁇ m or more, a sufficient energy density of the battery 2000 can be achieved. In the case where the thickness of the negative electrode 203 is 500 ⁇ m or less, the battery 2000 can operate at a high power.
  • At least one selected from the group consisting of the positive electrode 201 , the electrolyte layer 202 and the negative electrode 203 may contain a binder for the purpose of improving the adhesion between particles.
  • the binder is used to improve the binding properties of the materials of the electrodes.
  • binder examples include polyvinylidene fluoride, polytetrafluoroethylene, polyethylene, polypropylene, aramid resin, polyamide, polyimide, polyamide-imide, polyacrylonitrile, polyacrylic acid, polyacrylic acid methyl ester, polyacrylic acid ethyl ester, polyacrylic acid hexyl ester, polymethacrylic acid, polymethacrylic acid methyl ester, polymethacrylic acid ethyl ester, polymethacrylic acid hexyl ester, polyvinyl acetate, polyvinylpyrrolidone, polyether, polyethersulfone, hexafluoropolypropylene, styrene-butadiene rubber, and carboxymethylcellulose.
  • the binder can also be used a copolymer of two or more materials selected from the group consisting of tetrafluoroethylene, hexafluoroethylene, hexafluoropropylene, perfluoroalkyl vinyl ether, vinylidene fluoride, chlorotrifluoroethylene, ethylene, propylene, pentafluoropropylene, fluoromethyl vinyl ether, acrylic acid, and hexadiene. Moreover, a mixture of two or more selected from these may also be used.
  • At least one of the positive electrode 201 and the negative electrode 203 may contain a conductive additive for the purpose of improving the electronic conductivity.
  • the conductive additive include: graphites such as natural graphite and artificial graphite; carbon blacks such as acetylene black and Ketjenblack; conductive fibers such as a carbon fiber and a metal fiber; metal powders such as a fluorinated carbon powder and an aluminum powder; conductive whiskers such as a zinc oxide whisker and a potassium titanate whisker; conductive metal oxides such as titanium oxide; and conductive polymer compounds such as polyaniline compound, polypyrrole compound, and polythiophene compound.
  • a conductive carbon additive as the conductive additive can seek cost reduction.
  • the shape of the battery 2000 of Embodiment 2 is, for example, a coin type, a cylindrical type, a prismatic type, a sheet type, a button type, a flat type, or a stack type.
  • the battery 2000 of Embodiment 2 may be manufactured, for example, by preparing each of the positive electrode material 1000 of Embodiment 1, a material for forming an electrolyte layer, and a material for forming a negative electrode, and producing by a known method a stack in which a positive electrode, the electrolyte layer, and the negative electrode are disposed in this order.
  • Embodiment 3 will be described below. The description overlapping with that of Embodiment 2 will be omitted as appropriate.
  • FIG. 4 is a cross-sectional view schematically showing the configuration of a battery 3000 of Embodiment 3.
  • the battery 3000 of Embodiment 3 includes the positive electrode 201 , the electrolyte layer 202 , and the negative electrode 203 .
  • the positive electrode 201 includes the positive electrode material 1000 of Embodiment 1.
  • the electrolyte layer 202 is disposed between the positive electrode 201 and the negative electrode 203 .
  • the electrolyte layer 202 includes a first electrolyte layer 301 and a second electrolyte layer 302 .
  • the first electrolyte layer 301 is in contact with the positive electrode 201
  • the second electrolyte layer 302 is in contact with the negative electrode 203 .
  • the first electrolyte layer 301 may include a material that is the same as the first solid electrolyte material 111 .
  • the first solid electrolyte material 111 having excellent oxidation resistance in the first electrolyte layer 301 in contact with the positive electrode 201 By including the first solid electrolyte material 111 having excellent oxidation resistance in the first electrolyte layer 301 in contact with the positive electrode 201 , oxidative decomposition of the first electrolyte layer 301 can be suppressed, thereby suppressing an increase in internal resistance of the battery 3000 during charge.
  • the second electrolyte layer 302 may include a material that is different from the first solid electrolyte material 111 .
  • the reduction potential of the solid electrolyte material included in the first electrolyte layer 301 may be lower than the reduction potential of the solid electrolyte material included in the second electrolyte layer 302 .
  • the solid electrolyte material included in the first electrolyte layer 301 can be used without being reduced. As a result, the charge and discharge efficiency of the battery 3000 can be improved.
  • the second electrolyte layer 302 may include a sulfide solid electrolyte.
  • the reduction potential of the sulfide solid electrolyte included in the second electrolyte layer 302 is lower than the reduction potential of the solid electrolyte material included in the first electrolyte layer 301 .
  • the solid electrolyte material included in the first electrolyte layer 301 can be used without being reduced. As a result, the charge and discharge efficiency of the battery 3000 can be improved.
  • each of the first electrolyte layer 301 and the second electrolyte layer 302 may be 1 ⁇ m or more and 300 ⁇ m or less. In the case where the thickness of each of the first electrolyte layer 301 and the second electrolyte layer 302 is 1 ⁇ m or more, a short circuit between the positive electrode 201 and the negative electrode 203 is less likely to occur. In the case where the thickness of each of the first electrolyte layer 301 and the second electrolyte layer 302 is 300 ⁇ m or less, the battery 3000 can operate at a high power.
  • NCM Li(Ni, Co, Mn)O 2
  • NOBILTA manufactured by Hosokawa Micron Corporation
  • a compositing process at 6000 rpm for 30 minutes.
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 1 and the second electrolyte material Li 3 YBr 2 Cl 4 were weighed at a mass ratio of 81.55:18.45 and mixed in a mortar. Thus, a positive electrode material of Example 1 was produced.
  • NCM which is a positive electrode active material and the first solid electrolyte material of Example 2 were weighed at a mass ratio of 100:3. These materials were put into a dry particle composing machine, NOBILTA (manufactured by Hosokawa Micron Corporation) and subjected to a compositing process at 6000 rpm for 30 minutes. Thus, a positive electrode active material whose surface is coated with the first solid electrolyte material of Example 2 was obtained.
  • NOBILTA manufactured by Hosokawa Micron Corporation
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 2 and the second electrolyte material Li 3 YBr 2 Cl 4 were weighed at a mass ratio of 81.55:18.45 and mixed in a mortar. Thus, a positive electrode material of Example 2 was produced.
  • NCM which is a positive electrode active material and the first solid electrolyte material of Example 3 were weighed at a mass ratio of 100:3. These materials were put into a dry particle composing machine, NOBILTA (manufactured by Hosokawa Micron Corporation) and subjected to a compositing process at 6000 rpm for 30 minutes. Thus, a positive electrode active material whose surface is coated with the first solid electrolyte material of Example 3 was obtained.
  • NOBILTA manufactured by Hosokawa Micron Corporation
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 3 and the second electrolyte material Li 3 YBr 2 Cl 4 were weighed at a mass ratio of 81.55:18.45 and mixed in a mortar. Thus, a positive electrode material of Example 3 was produced.
  • NCM which is a positive electrode active material and the first solid electrolyte material of Example 4 were weighed at a mass ratio of 100:3. These materials were put into a dry particle composing machine, NOBILTA (manufactured by Hosokawa Micron Corporation) and subjected to a compositing process at 6000 rpm for 30 minutes. Thus, a positive electrode active material whose surface is coated with the first solid electrolyte material of Example 4 was obtained.
  • NOBILTA manufactured by Hosokawa Micron Corporation
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 4 and the second electrolyte material Li 3 YBr 2 Cl 4 were weighed at a mass ratio of 81.55:18.45 and mixed in a mortar. Thus, a positive electrode material of Example 4 was produced.
  • the positive electrode active material NCM and the second electrolyte material Li 3 YBr 2 Cl 4 were weighed at a mass ratio of 81.55:18.45 and mixed in a mortar. Thus, a positive electrode material of Comparative Example 1 was produced.
  • Respective batteries were produced by using the positive electrode materials of Examples 1 to 4 and Comparative Example 1 described above through the following steps.
  • metal In, metal Li, metal In, metal Li, and metal In were stacked in this order.
  • the metal In used had a thickness of 200 ⁇ m
  • the metal Li used had a thickness of 200 ⁇ m.
  • These stacked metals were pressure-molded at a pressure of 80 MPa to produce a stack composed of the positive electrode, the solid electrolyte layer, and a negative electrode.
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 1 and the second electrolyte material Li 2 S—P 2 S 5 were weighed at a mass ratio of 81.2:18.8 and mixed in a mortar. Thus, a positive electrode material of Example 5 was produced.
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 2 and the second electrolyte material Li 2 S—P 2 S 5 were weighed at a mass ratio of 81.2:18.8 and mixed in a mortar. Thus, a positive electrode material of Example 6 was produced.
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 3 and the second electrolyte material Li 2 S—P 2 S 5 were weighed at a mass ratio of 81.2:18.8 and mixed in a mortar. Thus, a positive electrode material of Example 7 was produced.
  • the positive electrode active material whose surface is coated with the first solid electrolyte material of Example 4 and the second electrolyte material Li 2 S—P 2 S 5 were weighed at a mass ratio of 81.2:18.8 and mixed in a mortar. Thus, a positive electrode material of Example 8 was produced.
  • the positive electrode active material NCM and the second electrolyte material Li 2 S—P 2 S 5 were weighed at a mass ratio of 81.2:18.8 and mixed in a mortar. Thus, a positive electrode material of Comparative Example 2 was produced.
  • Respective batteries were produced by using the positive electrode materials of Examples 5 to 8 and Comparative Example 2 described above through the following steps.
  • metal In, metal Li, metal In, metal Li, and metal In were stacked in this order.
  • the metal In used had a thickness of 200 ⁇ m
  • the metal Li used had a thickness of 200 ⁇ m.
  • These stacked metals were pressure-molded at a pressure of 80 MPa to produce a stack composed of the positive electrode, the solid electrolyte layer, and a negative electrode.
  • a charge test was performed by using the respective batteries of Examples 1 to 8 and Comparative Examples 1 and 2 described above under the following conditions.
  • the battery was placed in a thermostatic chamber at 85° C.
  • Constant-current charge was performed at a current value of 140 ⁇ A at 0.05 C rate (20-hour rate) with respect to the theoretical capacity of the battery.
  • the end-of-charge voltage was set to a voltage of 3.68 V (4.3 V vs. Li/Li + ).
  • constant-voltage charge was performed at a voltage of 3.68 V (4.3 V vs. Li/Li + ).
  • the end-of-charge current was set to a current value of 28 ⁇ A at 0.01 C rate (100-hour rate).
  • the battery was stored in a thermostatic chamber at 85° C. for 72 hours.
  • Table 1 shows the respective resistance values of the positive electrodes of Examples 1 to 8 and Comparative Examples 1 and 2.
  • Example 1 Li 3 Ti 0.5 Mg 0.5 F 6 Li 3 YBr 2 Cl 4 13.0
  • Example 2 Li 3 Ti 0.5 Ca 0.5 F 6 Li 3 YBr 2 Cl 4 40.3
  • Example 3 Li 2.6 Ti 0.4 Al 0.6 F 6 Li 3 YBr 2 Cl 4 9.6
  • Example 4 Li 3 Ti 0.5 Zr 0.5 F 7 Li 3 YBr 2 Cl 4 47.9 Comparative Not included Li 3 YBr 2 Cl 4 72.2
  • Example 5 Li 3 Ti 0.5 Mg 0.5 F 6 Li 2 S—P 2 S 5 5.8
  • Example 6 Li 3 Ti 0.5 Ca 0.5 F 6 Li 2 S—P 2 S 5 25.7
  • Example 7 Li 2.6 Ti 0.4 Al 0.6 F 6 Li 2 S—P 2 S 5 1.2
  • Example 8 Li 3 Ti 0.5 Zr 0.5 F 7 Li 2 S—P 2 S 5 54.6 Comparative Not included Li 2 S—P 2 S 5 356
  • Example 2 Li 3 Ti 0.5 Mg 0.5 F 6 Li 3 YBr 2 Cl 4
  • the battery of Example 1 exhibits a low resistance of the positive electrode.
  • the reasons are as follows; since the first solid electrolyte material having high oxidation resistance coats at least partially the surface of the positive electrode active material, a contact between the positive electrode active material and Li 3 YBr 2 Cl 4 , which is the second electrolyte material, is suppressed, so that an increase in resistance of the positive electrode is suppressed.
  • the battery which was formed using the positive electrode material including the positive electrode active material whose surface is not coated with the first solid electrolyte material, exhibits a high resistance value of 72.2 ⁇ .
  • Example 1 As indicated by the results of Examples 2 to 4, even in the case where M1 included in the first solid electrolyte material is Ca, Al, or Zr, a low resistance of the positive electrode can be exhibited as in Example 1.
  • the battery of the present disclosure can be utilized, for example, as an all-solid-state lithium-ion secondary battery.

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